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Prolongation of electrode lifetime in biofuel cells by periodic enzyme renewal

  • Bioenergy and Biofuels
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Abstract

Enzymatically catalyzed biofuel cells show unique specificity and promise high power densities, but suffer from a limited lifetime due to enzyme deactivation. In the present work, we demonstrate a novel concept to extend the lifetime of a laccase-catalyzed oxygen reduction cathode in which we decouple the electrode lifetime from the limited enzyme lifetime by a regular resupply of fresh enzymes. Thereto, the adsorption behavior of laccase from Trametes versicolor to buckypaper electrode material, as well as its time-dependent deactivation characteristics, has been investigated. Laccase shows a Langmuir-type adsorption to the carbon nanotube-based buckypaper electrodes, with a mean residence time of 2 days per molecule. In a citrate buffer of pH 5, laccase does not show any deactivation at room temperature for 2 days and exhibits a half-life of 9 days. In a long-term experiment, the laccase electrodes were operated at a constant galvanostatic load. The laccase-containing catholyte was periodically exchanged against a freshly prepared one every second day to provide sufficient active enzymes in the catholyte for the replacement of desorbed inactive enzymes. Compared to a corresponding control experiment without catholyte exchange, this procedure resulted in a 2.5 times longer cathode lifetime of 19 ± 9 days in which the electrode showed a potential above 0.744 V vs. normal hydrogen electrode at 110 μA cm−2. This clearly indicates the successful exchange of molecules by desorption and re-adsorption and is a first step toward the realization of a self-regenerating enzymatic biofuel cell in which enzyme-producing microorganisms are integrated into the electrode to continuously resupply fresh enzymes.

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Acknowledgments

The authors gratefully acknowledge financial support by the German Research Foundation (DFG) through the PhD program “Micro Energy Harvesting” (GRK 1322) and the German Ministry of Education and Research (BMBF) under the program Bioenergie2021 (grant no. 03SF0382). Furthermore, we would like to thank Dr. Daniel Wohlwend (Laboratory for Biochemistry) for his assistance in understanding laccase unfolding.

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Author notes

  1. J. Kestel

    Present address: ifm electronic GmbH, Essen, Germany

Authors and Affiliations

  1. Laboratory for MEMS Applications, Department of Microsystems Engineering—IMTEK, University of Freiburg, Georges-Koehler-Allee 103, 79110, Freiburg, Germany

    S. Rubenwolf, S. Sané, J. Kestel, F. von Stetten, R. Zengerle & S. Kerzenmacher

  2. Freiburg Materials Research Centre (FMF), University of Freiburg, Freiburg, Germany

    L. Hussein, G. Urban & M. Krueger

  3. Laboratory for Sensors, Department of Microsystems Engineering—IMTEK, University of Freiburg, Georges-Koehler-Allee 103, 79110, Freiburg, Germany

    L. Hussein, G. Urban & M. Krueger

  4. BIOSS Centre for Biological Signalling Studies, University of Freiburg, Freiburg, Germany

    R. Zengerle

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  1. S. Rubenwolf
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  2. S. Sané
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Correspondence to S. Kerzenmacher.

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Rubenwolf, S., Sané, S., Hussein, L. et al. Prolongation of electrode lifetime in biofuel cells by periodic enzyme renewal. Appl Microbiol Biotechnol 96, 841–849 (2012). https://doi.org/10.1007/s00253-012-4374-8

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  • DOI: https://doi.org/10.1007/s00253-012-4374-8

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